Abstract
We report on multidimensional spectroscopy in the mid-infrared, performed using a calomel-based acousto-optic programmable dispersive filter. Although the associated spectral resolution is currently not as good as what has been previously reported using time-domain interferometers or other pulse-shaping technologies, the extreme compactness of the calomel crystal allows a straightforward implementation in a pre-existing pump-probe setup. Furthermore, the frequency-domain approach allows easy measurement of 2D slices of the multidimensional spectrum associated with a given pump frequency. We demonstrate our method with the measurement of the mid-infrared spectrum of carboxy-hemoglobin in three spectro-temporal dimensions.
Highlights
Two-dimensional infrared (2DIR) spectroscopy has been established in the last two decades as the most advanced form of femtosecond vibrational spectroscopy
We report on the first application of a calomel acousto-optic programmable dispersive filter (AOPDF) for 2DIR spectroscopy
With the AOPDF removed and mirror M located in a position suitable for reflecting dotted-line beam (1), the setup shown in Fig. 1 is merely a standard pump-probe setup
Summary
Two-dimensional infrared (2DIR) spectroscopy has been established in the last two decades as the most advanced form of femtosecond vibrational spectroscopy. It shares many conceptual and experimental aspects with the other form of multidimensional spectroscopy, namely two-dimensional electronic spectroscopy (2DES) [2], which is a powerful tool for investigating electronic structure and dynamics using visible or ultra-violet femtosecond pulses. In the frequency-domain approach [3], the measured signal is recorded as a function of the center frequency of a tunable narrow-band pump pulse, e.g. using a Fabry-Perot etalon. In the time-domain (or Fourier-transform) approach, the pump-probe signal is recorded as a function of the time delay between two broadband pump pulses, yielding the exciting pump frequency by Fourier-transform spectroscopy [2, 8]
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